The current research focuses on removal of arsenite ions from aqueous solutions by a new adsorbent, surfactant modified akaganeite (Ak(m)), prepared after the adsorption of the cationic surfactant, hexadecyl trimethyl ammonium bromide (N-Cetyl-N,N,N-Trimethylammonium Bromide) onto akaganeite. The new adsorbent was investigated with Fourier transform infrared spectra and X-ray photoelectron spectroscopy methods for a better understanding of the effects of surface properties on arsenite adsorption. Surfactant modified akaganeite was found to be an effective adsorbent for the removal of arsenite ions from aqueous systems. It presented a significantly higher arsenite adsorption capacity than the pure nanocrystalline akaganeite. Kinetics of adsorption obeys a second-order rate equation. The maximum adsorption capacity was found to 328.3 mg g(-1) over a wide pH range significantly higher than those of other adsorbents reported.